JP4364529B2 - Oxygen isotope enrichment method and apparatus - Google Patents

Description

【００３２】
次に、原料酸素として通常の高純度酸素を使用し、１年間で１０ｋｇ（Ｈ_２Ｏ換算）製造する場合の各経路におけるプロセス流量等の計算値を表２に示す。ターゲットのアイソトポマーには、^１６Ｏ^１６Ｏ^１７Ｏを選択した。このターゲットのアイソトポマーを分解するための光には、波長が９９２ｎｍのレーザー光を使用した。レーザー出力は２．２Ｗ、吸収断面積は３．０×１０^−２３ｃｍ^２とした。また、光反応セルの圧力は１３ｋＰａ（１００Torr）、温度は１５０Ｋとした。光路長は４０ｍ、滞留時間は１００秒、光の利用率は０．０００３、ターゲットのアイソトポマーの収率は０．９０、ターゲットのアイソトポマーの分解と同時に発生する他のアイソトポマーの非選択的分解量は、ターゲットのアイソトポマーの１に対して１０とした。このときの^１７Ｏの濃縮率は８５．４となった。また、オゾナイザーの消費電力は６．７ｋＷであった。
【００３３】
【表２】

【００３４】
【発明の効果】
以上説明したように、本発明によれば、酸素同位体を分離濃縮するための手段としてオゾンの光分解反応を選択したことにより、酸素の安定同位体である^１７Ｏや^１８Ｏを効率よく濃縮することができる。
【図面の簡単な説明】
【図１】 オゾンの吸収スペクトルを示す図である。
【図２】 本発明方法を実施するための装置構成例を示すブロック図である。
【図３】 図である。
【符号の説明】
１１…オゾン生成手段、１２…オゾン分離手段、１３…オゾン分解手段、１４…酸素分離手段、１５…第２オゾン分解手段、１６…第２酸素分離手段、２１…オゾナイザー、２２…第１蒸留塔、２３…凝縮器、２４…リボイラー、２５…熱交換器、２６…バッファタンク、２７…ブロワー、３１…光源、３２…光反応セル、３３…第２蒸留塔、３４…凝縮器、３５…リボイラー、３６…熱交換器[0001]
BACKGROUND OF THE INVENTION
The present invention relates to an oxygen isotope enrichment method and apparatus, and more particularly, selectively enriches ¹⁷ O and ¹⁸ O, which are stable isotopes of oxygen having a very small abundance ratio, by utilizing a decomposition reaction of ozone by light. The present invention relates to a method and an apparatus.
[0002]
[Prior art]
The oxygen isotopes ¹⁷ O and ¹⁸ O used as tracers in the diagnosis of adult diseases and the like have a very small abundance ratio in the natural world, and therefore need to be separated and concentrated for use. As the concentration method of the ^{18 O,} by selectively photolysis those comprising ^{18 O} by irradiating a laser beam to saturated chain ethers, a method of obtaining a product containing ^{18 O} is known (e.g., (See Patent Document 1). In addition, there is a method of selectively concentrating ¹⁸ O by irradiating a laser beam to aldehyde or carbon monoxide.
[0003]
[Patent Document 1]
Japanese Examined Patent Publication No. 6-102134
[Problems to be solved by the invention]
However, in the conventional method, the concentration rate is low, the utilization efficiency of light contributing to the reaction is low, or the oscillation energy efficiency of the laser light is low, and further post-processing for extracting the concentrated chemical species However, it was not established industrially. On the other hand, it has also been proposed to concentrate oxygen isotopes by distillation, but there is a problem that the startup time of the apparatus becomes extremely long in order to increase the concentration.
[0005]
Therefore, the present invention provides an oxygen isotope enrichment method and apparatus capable of concentrating ¹⁷ O and ¹⁸ O, which are stable isotopes of oxygen, in the state of oxygen, and which can be carried out with a simple apparatus configuration. It is intended to provide.
[0006]
To achieve the above object, a method of concentrating oxygen isotopes of the present invention basically is irradiated with light of a specific wavelength in the ozone, the ozone containing at least one of ^{17 O} and ^{18 O} in the molecule after decomposed into oxygen, in which ozone is separated and generates oxygen and non-decomposed by the decomposition of ozone, characterized by concentrating the at least one of the separated in oxygen ^{17 O} and ^{18 O} Specifically, an ozone generation step for generating ozone using oxygen as a raw material, an ozone separation step for separating ozone generated in the step from the raw material oxygen , and light having a specific wavelength in the ozone separated in the step irradiating the, ozone decomposition step of decomposing into oxygen ozone containing at least one of ^{17 O} and ^{18 O} in the molecule, the higher in the ozone undecomposed and oxygen ozone generated by decomposing該工separated And acid It is characterized by containing oxygen separation step of concentrating the at least one of ^{17 O} and ^{18 O} in.
[0007]
Furthermore, the ozone separated in the oxygen separation step is irradiated with light having a specific wavelength different from that in the ozone decomposition step, and is ozone different from ozone decomposed in the ozone decomposition step, and at least of ¹⁷ O and ¹⁸ O A second ozone decomposing step of selectively decomposing ozone containing one of the molecules into oxygen, and oxygen generated by decomposing ozone in the step and undecomposed ozone are separated into ¹⁷ O in oxygen. And a second oxygen separation step of concentrating at least one of ¹⁸ O, and different oxygen isotopes can be concentrated in two stages.
[0008]
Examples of the isotopomer of ozone include ¹⁶ O ¹⁶ O ¹⁶ O, ¹⁶ O ¹⁶ O ¹⁷ O, ¹⁶ O ¹⁷ O ¹⁶ O, ¹⁶ O ¹⁶ O ¹⁸ O, and ¹⁶ O ¹⁸ O ¹⁶ from the types of oxygen isotopes and combinations thereof. O, ¹⁶ O ¹⁷ O ¹⁷ O, ¹⁷ O ¹⁶ O ¹⁷ O, ¹⁶ O ¹⁷ O ¹⁸ O, ¹⁷ O ¹⁶ O ¹⁸ O, ¹⁶ O ¹⁸ O ¹⁷ O, ¹⁷ O ¹⁷ O ¹⁷ O, ¹⁶ O ¹⁸ O ¹⁸ O ¹⁸ O ¹⁶ O ¹⁸ O, ¹⁷ O ¹⁷ O ¹⁸ O, ¹⁷ O ¹⁸ O ¹⁷ O, ¹⁷ O ¹⁸ O ¹⁸ O, ¹⁸ O ¹⁷ O ¹⁸ O, ¹⁸ O ¹⁸ O ¹⁸ O Become.
[0009]
In the present invention, specific light of ozone is decomposed to generate oxygen containing oxygen isotopes by irradiating ozone light containing these various isotopomers with specific light. For example, when an isotopomer of ¹⁶ O ¹⁶ O ¹⁷ O is decomposed by light irradiation, three molecules of oxygen are generated from two molecules of ozone according to the following reaction formulas (1) and (2).
[0010]
¹⁶ O ¹⁶ O ¹⁷ O + “light irradiation” → O ₂ + O (1)
O ₃ + O → 2O ₂ (2)
[0011]
In this reaction, ¹⁷ O contained in ozone decomposed by light irradiation in the reaction formula (1) is included in the generated “O ₂ ” or becomes “O”, and this “O” is immediately Since it reacts with other ozone by reaction formula (2) to become two molecules of oxygen, this ¹⁷ O exists in one molecule among the three molecules of oxygen generated by reaction formulas (1) and (2). Will do. As a result, ¹⁷ O is concentrated in oxygen decomposed by ozone. In addition, although the ozone which reacts in Reaction formula (2) may also contain ¹⁷ O and ¹⁸ O, the probability is very low and can be said to be a negligible amount.
[0012]
Moreover, the bond dissociation energy of ozone is 1.05 eV, and ozone decomposes in light absorption with a wavelength of 1.18 μm or less. The following bands are conventionally known as light absorption of ozone.
[0013]
Wulf band 700 ~ 1000nm (1.2 ~ 1.8eV) Near infrared
Chappius band 450 ~ 850nm (1.5 ~ 2.8eV) Visible range
Huggins band 300 ~ 360nm (3.4 ~ 4.1eV) UV
Hartly band 200-300nm (4.1-6.2eV) UV region [0014]
Among these bands, according to the literature (Journal of Chemical Physics vol.108 no.13 p.5449-5457), a sharp absorption as shown in FIG. 1 is observed in the vicinity of a wavelength of 1000 nm (wave number of 10,000 cm ⁻¹ ). A spectrum is observed. FIG. 1 shows light absorption in ¹⁶ O ₃ ( ¹⁶ O ¹⁶ O ¹⁶ O) and ¹⁸ O ₃ ( ¹⁸ O ¹⁸ O ¹⁸ O). The maximum peak of ¹⁶ O ₃ has a wavenumber of 10081 cm ⁻¹ (wavelength). 999.965 nm), and the maximum peak of ¹⁸ O ₃ is found to have a wave number of 10076 cm ⁻¹ (wavelength: 992.457 nm). Therefore, it can be seen that the wavelength at which ozone isotopomers containing ¹⁷ O and ¹⁸ O can be efficiently decomposed is between the two, and the desired ozone can be selectively decomposed by selecting the wavelength between them.
[0015]
Other absorption peaks can also be used, but the above range is optimal in view of ozone decomposition efficiency. In particular, the use of such near-infrared or visible light has the advantage of being easier to handle than using ultraviolet light. Furthermore, if high-energy ultraviolet light is used, not only the target ozone isotopomer but also other ozone isotopomers may be decomposed, resulting in a reduction in the concentration efficiency of oxygen isotopes. Become.
[0016]
If the light source is slightly deviated from the desired ozone decomposition wavelength and the selective decomposition efficiency is poor, the ozone absorption wavelength is shifted by the Stark effect by applying an electric field to the ozone when irradiating light. Therefore, it is possible to precisely match the absorption wavelength of ozone with the wavelength of the light source.
[0017]
As a light source for obtaining light of such a wavelength, sunlight spectroscopy, InGaAsP semiconductor laser or light emitting diode, AlGaInP semiconductor laser or light emitting diode, GaAsSb semiconductor laser or light emitting diode, CdZnTe semiconductor laser or light emitting diode CdZnSe-based semiconductor lasers or light emitting diodes, or dye lasers that can be optically pumped with a mercury lamp, YAG laser, Ar ion laser, Kr ion laser, or the like can be used.
[0018]
Furthermore, when irradiating light to ozone, in order to suppress the molecular collision as much as possible by lengthening the mean free path of ozone molecules, it is preferable to set the pressure under a low pressure, for example, 13 kPa (100 Torr) or less. Thereby, it is possible to prevent the absorption width of light from expanding due to molecular collision. Moreover, in order to suppress the natural decomposition | disassembly of ozone, it is preferable to cool not only the time of irradiating light to ozone but the whole system to low temperature, for example, the range of 100-250K. As a result, the absorption peak can be sharpened, and the concentration of oxygen containing oxygen isotopes can be improved by suppressing the generation of oxygen by natural decomposition.
[0019]
On the other hand, ozone can be easily generated by silently discharging oxygen as an ozone raw material with a general ozonizer or irradiating ultraviolet rays from a mercury lamp or the like. As the raw material oxygen, high-purity oxygen containing as little as possible impurities such as argon and nitrogen is desirable. However, if these impurities can be sufficiently separated when separating ozone and oxygen, an industrial having a purity of about 99.5% Oxygen for use can also be used as raw material oxygen. Further, oxygen or enriched for ^{17 O} and ^{18 O} in the concentration method of the present invention, the oxygen enriched for ^{17 O} and ^{18 O} in other concentration methods can also be used as a raw material oxygen. Further, the separation between ozone and oxygen can be easily carried out by low-temperature distillation using the difference between the boiling points of the two or low-temperature adsorption using the difference in the adsorptivity of the two to an adsorbent such as silica gel.
[0020]
For example, as shown in the block diagram of FIG. 2, the optimum apparatus configuration for carrying out the method of the present invention is generated by the ozone generating means 11 for generating ozone from the raw material oxygen GO and the ozone generating means. The ozone separation means 12 for separating the ozone OZ and the raw material oxygen, and the light L having a specific wavelength is irradiated to the ozone separated by the ozone separation means 12 to selectively convert ozone containing oxygen isotopes into oxygen. An ozone decomposing means 13 for decomposing, and an oxygen separating means 14 for separating oxygen OC generated by decomposing ozone by the ozone decomposing means 13 and undecomposed ozone OZ to concentrate oxygen isotopes in oxygen. It is a thing.
[0021]
Further, the ozone OZ separated by the oxygen separation means 14 is irradiated with light L, and ozone containing oxygen isotopes different from the ozone decomposed by the ozone decomposition means 13 is selectively decomposed into oxygen. Ozone decomposing means 15; second oxygen separating means 16 for separating oxygen OC2 generated by decomposing ozone by the second ozone decomposing means 15 and undecomposed ozone OZ2 to concentrate oxygen isotopes in oxygen; Can also be provided.
[0022]
Further, by providing a route for circulating and introducing the oxygen GO separated by the ozone separation means 12 into the ozone generation means 11, the consumption of raw material oxygen can be reduced. Further, the ozone decomposing means 13 is preferably provided with a cooling means and a decompression means.
[0023]
DETAILED DESCRIPTION OF THE INVENTION
FIG. 3 is a system diagram showing an embodiment of the oxygen isotope concentrator of the present invention. This concentrator first separates the ozone generator 21 which is an ozone generating means for generating ozone from raw material oxygen, and the ozone generated by the ozonizer 21 and the raw material oxygen as equipment for obtaining ozone from the raw material oxygen. A first distillation column 22 as an ozone separation means, a condenser 23 for providing the cooling required for the low-temperature distillation operation in the first distillation column 22, and an ascending gas in the first distillation column are generated. A reboiler 24; a heat exchanger 25 for recovering the cold of the first distillation column derived gas into the first distillation column introduction gas; a buffer tank 26 for temporarily storing the first distillation column derived gas; A blower 27 for circulating and introducing the first distillation column-derived gas into the ozonizer 21 is provided.
[0024]
As equipment for concentrating oxygen containing a specific isotope from ozone, a photoreaction cell 32 for decomposing a specific ozone isotopomer into oxygen by light irradiated from a light source 31, and a photoreaction cell 32 The second distillation column 33, which is an oxygen separation means for separating the separated oxygen and undecomposed ozone and concentrating oxygen isotopes in oxygen, and the cooling required for the low-temperature distillation operation in the second distillation column 33 A condenser 34 for supplying, a reboiler 35 for generating the rising gas in the second distillation column, and a heat exchanger 36 for recovering the cold of the second distillation column derived gas into the second distillation column introduction gas Is provided.
[0025]
The raw material oxygen supplied from the path 51 and joined with the oxygen circulated from the path 52 is partially ozonized by silent discharge in the ozonizer 21 and is cooled by the heat exchanger 25 as an ozone / oxygen mixed gas. , Is introduced into the middle stage of the first distillation column 22 from the path 53. This ozone / oxygen mixed gas is distilled by the reflux liquid generated in the condenser 23 at the upper part of the first distillation column and the rising gas generated in the reboiler 24 at the lower part of the first distillation column. Oxygen gas is separated into liquefied ozone at the bottom of the first distillation column 22. A part of the oxygen extracted from the upper part of the first distillation column into the path 54 is branched into the condenser 23, and the remaining part is temporarily stored in the buffer tank 26 through the path 55, and then compressed by the blower 27. 52 is introduced into the ozonizer 21 in a circulating manner.
[0026]
A part of the ozone extracted from the bottom of the first distillation column 22 to the path 56 is branched into the reboiler 24, and the rest is introduced into the photoreaction cell 32 in the form of gas through the valve 57. The specific isotopomer in the ozone is decomposed into oxygen by light emitted from the light source 31, and an ozone / oxygen mixed gas composed of decomposed oxygen and undecomposed ozone is led out from the path 58 through the valve 59. The inside of the photoreaction cell 32 is reduced to a pressure of 13 kPa or less and cooled to a range of 100 to 250 K in order to efficiently perform a specific ozone isotopomer decomposition in a stable state. The pressure and temperature can be appropriately set according to the decomposition state of ozone, and at least a predetermined pressure and a predetermined temperature between the valves 57 and 59 on both sides of the photoreaction cell 32 within a range where ozone does not liquefy or solidify. Try to keep on.
[0027]
The ozone / oxygen mixed gas in the path 58 is cooled by the heat exchanger 36 and then introduced into the middle stage of the second distillation column 33, and, similar to the first distillation column 22, the reflux liquid from the condenser 34, Distillation is performed by the rising gas from the reboiler 35, ozone is separated at the bottom of the tower, and oxygen gas containing specific isotope oxygen is concentrated at the top of the tower. The concentrated specific isotope-containing oxygen gas is extracted from the upper part of the second distillation column 33 to the path 61 and partially branched to the condenser 34, and then recovered as a product from the path 62. A part of the ozone extracted from the bottom of the second distillation column 33 to the path 63 is branched to the reboiler 35, and then extracted to the path 64 through the heat exchanger 36.
[0028]
The ozone in the path 64 is normally decomposed into oxygen by an ozone decomposing means using a catalyst or the like and discharged. In addition, the ozone in this path 64 is introduced into a second photoreaction cell as a second ozone decomposing means provided separately from the photoreaction cell 32, and an isotopomer different from that decomposed in the photoreaction cell 32 is obtained. The isotope-containing oxygen produced by the decomposition can be separated and concentrated from ozone using a distillation column or the like as the second oxygen separation means.
[0029]
The operating conditions of each distillation column are arbitrary, but the concentration of the isotope-containing oxygen gas decreases when oxygen enters the photoreaction cell, so that ozone in a state that does not contain oxygen as much as possible is obtained. Is preferred. Moreover, nitrogen and argon of suitable temperature can be used for the cold source supplied to a condenser and the heating source supplied to a reboiler. Furthermore, nitrogen and argon at an appropriate temperature can be used for cooling the photoreaction cell, and a vacuum pump can be installed in an appropriate path downstream from the photoreaction cell for reducing the pressure in the system including the photoreaction cell. Or by liquefying and depressurizing with liquefied nitrogen or the like. Moreover, what is necessary is just to select the material which does not have the reactivity with respect to ozone, or a catalytic action as a material of each apparatus, Usually, it is preferable to use glass, a fluororesin (polytetrafluoroethylene), etc.
[0030]
Table 1 shows the calculated values of the process flow rate and the like in each route when ¹⁷ O is concentrated using the concentrator having the configuration shown in FIG. 3 and 10 kg (in terms of H ₂ O) is produced in one year. As raw material oxygen, oxygen gas in which ¹⁷ O and ¹⁸ O were concentrated by a distillation method was used. ¹⁶ O ¹⁷ O ¹⁸ O was selected as the target isotopomer to be decomposed in the photoreaction cell. Laser light having a wavelength of 992 nm was used as light for decomposing the isotopomer of the target. The laser output was 1.0 W and the absorption cross section was 3.0 × 10 ⁻²³ cm ² . The pressure of the photoreaction cell was 13 kPa (100 Torr) and the temperature was 200K. The optical path length is 40 m, the residence time is 100 seconds, the light utilization rate is 0.0019, the target isotopomer yield is 0.90, and the non-selective degradation amount of other isotopomers generated simultaneously with the target isotopomer degradation is 3.3 for 1 of the target isotopomer. At this time, the concentration ratio of ¹⁷ O was 10.8. The power consumption of the ozonizer was 3.0 kW.
[0031]
[Table 1]

[0032]
Next, Table 2 shows calculated values such as process flow rate in each route when normal high purity oxygen is used as raw material oxygen and 10 kg (H ₂ O conversion) is produced in one year. ¹⁶ O ¹⁶ O ¹⁷ O was selected as the target isotopomer. Laser light having a wavelength of 992 nm was used as light for decomposing the isotopomer of the target. The laser output was 2.2 W and the absorption cross section was 3.0 × 10 ⁻²³ cm ² . The pressure of the photoreaction cell was 13 kPa (100 Torr) and the temperature was 150K. The optical path length is 40 m, the residence time is 100 seconds, the light utilization rate is 0.0003, the target isotopomer yield is 0.90, and the non-selective degradation amount of other isotopomers generated simultaneously with the target isotopomer degradation is , 10 for 1 of the target isotopomer. At this time, the concentration ratio of ¹⁷ O was 85.4. The power consumption of the ozonizer was 6.7 kW.
[0033]
[Table 2]

[0034]
【The invention's effect】
As described above, according to the present invention, by selecting the photolysis reaction of ozone as a means for separating and concentrating oxygen isotopes, the oxygen stable isotopes ¹⁷ O and ¹⁸ O are efficiently concentrated. can do.
[Brief description of the drawings]
FIG. 1 is a diagram showing an absorption spectrum of ozone.
FIG. 2 is a block diagram showing a configuration example of an apparatus for carrying out the method of the present invention.
FIG. 3 is a diagram.
[Explanation of symbols]
DESCRIPTION OF SYMBOLS 11 ... Ozone production | generation means, 12 ... Ozone separation means, 13 ... Ozone decomposition means, 14 ... Oxygen separation means, 15 ... 2nd ozone decomposition means, 16 ... 2nd oxygen separation means, 21 ... Ozonizer, 22 ... 1st distillation column 23 ... Condenser, 24 ... Reboiler, 25 ... Heat exchanger, 26 ... Buffer tank, 27 ... Blower, 31 ... Light source, 32 ... Photoreaction cell, 33 ... Second distillation column, 34 ... Condenser, 35 ... Reboiler 36 ... Heat exchanger

Claims (11)

Ozone was irradiated with light of a particular wavelength, after decomposing the oxygen ozone containing at least one of ^{17 O} and ^{18 O} in the molecule, and ozone of oxygen and non-decomposed ozone generated by decomposition A method for concentrating oxygen isotopes, comprising separating and concentrating at least one of ¹⁷ O and ¹⁸ O in the separated oxygen. An ozone generation step for generating ozone using oxygen as a raw material, an ozone separation step for separating the ozone generated in the step from the raw material oxygen, and the ozone separated in the step are irradiated with light of a specific wavelength , and ¹⁷ in the molecule. an ozone decomposition step of decomposing into oxygen ozone containing at least one of O and ^{18 O,} the ozone separates the oxygen and undecomposed ozone generated by decomposing oxygen in about該工 ^{17 O} and ^And an oxygen separation step of concentrating at least one of ¹⁸ O. The ozone separated in the oxygen separation step is irradiated with light having a specific wavelength different from that in the ozone decomposition step, and is ozone different from ozone decomposed in the ozone decomposition step, and at least one of ¹⁷ O and ¹⁸ O one and a second ozone decomposition step of decomposing ozone containing in the molecule the oxygen,該工more ozone is generated oxygen and non-decomposed by decomposing the ozone into separated oxygen ^{17 O} and ^{18 O} A method for concentrating oxygen isotopes according to claim 2, further comprising a second oxygen separation step of concentrating at least one of them . The specific wavelength, characterized in that it is a near-infrared region or a wavelength different from the wavelength of the light absorption peak of a is either visible noise deviation ¹⁶ O ₃ in the range of 450~850nm ranging 700~1000nm The oxygen isotope enrichment method according to any one of claims 1 to 3 . The oxygen isotope enrichment method according to any one of claims 1 to 3, wherein the specific wavelength is in a range of 991.965 to 992.457 nm . The oxygen isotope enrichment method according to any one of claims 1 to 3, wherein the ozone absorption wavelength is adjusted by applying an electric field when the ozone is irradiated with light having a specific wavelength. . The irradiation of light of a particular wavelength to the ozone, temperature 100～250K, method for concentrating oxygen isotopes according to any one of claims 1 to 3, characterized in that in the following pressure 13 kPa. Ozone generating means for generating ozone from raw oxygen, ozone separating means for separating ozone generated by the ozone generating means and raw oxygen, and irradiating light of a specific wavelength to the ozone separated by the ozone separating means; and ozone decomposing means for decomposing the ozone into oxygen containing at least one of ^{17 O} and ^{18 O} in the molecule, and separating the ozone of oxygen and non-decomposed ozone generated by decomposition in the ozone decomposing means An oxygen isotope concentrating apparatus, comprising: an oxygen separation means for concentrating at least one of ¹⁷ O and ¹⁸ O in oxygen. Irradiating light of different specific wavelengths and the ozone decomposing means ozone separated in the oxygen separation unit, whereas at least one of a and ^{17 O} and ^{18 O} different ozone and ozone decomposition in the ozone decomposition step a second ozone decomposing means for decomposing ozone containing in the molecule the oxygen and by separating the ozone of oxygen and non-decomposed ozone generated by decomposition in the second ozone decomposing means during oxygen ^{17 O} and The oxygen isotope concentrating apparatus according to claim 8, further comprising a second oxygen separation unit that concentrates at least one of ¹⁸ O. 9. The oxygen isotope concentrator according to claim 8 , further comprising a path for circulatingly introducing the raw material oxygen separated by the ozone separation unit into the ozone generation unit. 9. The oxygen isotope concentrator according to claim 8 , wherein the ozonolysis means comprises a cooling means and a decompression means.

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